CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Qiao Zhang,Chunxi Hai,Zhiqiang Zhu,Xuemei Zhuo,Yanxia Sun,Shengde Dong,Luxiang Ma,Xin He,Qi Xu,Yuan Zhou
The layer-structured titanium oxide lithium ion sieve (TiO 2 ·H 2 O) is regarded as one of the most promising adsorbents for recovering Li + from low-grade brines with high Mg 2+ /Li + ratios and low lithium concentrations. This is due to its exceptional theoretical lithium adsorption capacity and outstanding stability. Nevertheless, its prolonged adsorption equilibrium time, frequently in excess of 72 h, has constrained its large-scale practical application, thus confining its utilization primarily to laboratory settings. To address this challenge, we have developed a Ce-doped TiO 2 ·H 2 O adsorbent through a simple in-situ calcination method. The as-prepared adsorbents have been shown to achieve a high adsorption capacity of up to 58.42 mg/g within 10 h in a 700 ppm LiOH solution, while exhibiting a very low Ti 4+ dissolution loss rate of around 0.6 %. It is noteworthy that the Ce doping process resulted in a 14 % enhancement in adsorption capacity, accompanied by a substantial improvement in the desorption/adsorption kinetics and selectivity of the TiO 2 ·H 2 O lithium adsorbents. In summary, this study presents a novel methodology for accelerating the Li + sorption in Ti–O frameworks derived from natural brines, which provides valuable insights for enhancing the practical applicability of TiO 2 ·H 2 O.
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产品关联
DOI
高影响因子
ChemSusChem
·
2025
·Vol. 18
·期 20
·e202501351
·
IF 6.6
Tianhua Chen,Yongzheng Zhang,Simeng Wang,Jin Li,Hongzhen Lin,Dusan Losic,Shimou Chen,Jian Wang
Solid-state lithium metal batteries (SSLMBs) are promising for realizing higher energy density. However, the poor interfacial Li + transport kinetics and Li dendrite growth inhibit SSLMBs, leading to sluggish interfacial ion diffusion and depressive lifespan, which is attributed to high barriers blocked by anions or interface space in solid-state electrolytes. Herein, a flexible solid-state polymer skeleton employed with ionic liquid and metal-organic frameworks (PIM) electrolyte is proposed to strengthen interfacial Li ion exchange by improving the Li + sieving effect and interfacial wettability. Thanks to the immobilization effect of TFSI − anions affected by positive metal atom centers and pore morphology, the PIM electrolyte exhibits exceptional properties, i.e., a high ionic conductivity up to 3.1 mS cm −1 at 60 °C and an improved Li + transference number of 0.65, enabling symmetric cells of Li metal to run steadily for over 1000 h with lower voltage hysteresis (25 mV). Meanwhile, matching with high-voltage electrodes, the solid-state PIM electrolyte exhibits good compatibility and stability toward LiNi 0.6 Co 0.2 Mn 0.2 O 2 and LiFePO 4 electrodes, showing the capacity retentions of 85.5% and 96.5% after 120 and 400 cycles, respectively. This work suggests low interfacial diffusion resistances and high compatibility for make it a promising candidate for future solid-state battery. Graphical An ion-selective SSE is proposed with an accelerated Li+ migration feature, where the metal organic framework functions as a molecular sieve to selectively block bulky anions and the ionic liquid acts as Li ion bridge. Consequently, The as-prepared full cell exhibited high capacity and retention under the upper voltage of 4.3 V.
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产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Zhenguo Wang,Tingting Chen,Zhiwen Zheng,Bocheng Su,Kangwei Wen,Lin Qin,Changqing Song,Binbin Liu,Haihong Yin
Lithium–sulfur batteries (LSBs) are regarded as a competitive candidate for future energy storage systems due to their exceptionally high theoretical capacity and energy density, but their practical use is limited by severe lithium polysulfides (LiPSs) shuttling and uncontrolled lithium dendrite growth, harming cycling stability and Coulombic efficiency. Herein, a multifunctional Ce-ZIF-8/PDA@PP separator is fabricated via in situ growth. Theoretical and experimental studies confirm it integrates synergistic functionalities from polydopamine (PDA), ZIF-8, and Ce doping. The PDA interlayer, rich in polar groups, enhances electrolyte wettability, homogenizes Li+ flux, acts as a chemical anchor and nucleation facilitator, enabling uniform Ce-ZIF-8 growth on inert PP. ZIF-8 provides uniform microporous channels for size-selective Li+ transport and LiPSs anchoring sites. Redox-active Ce3+/Ce4+ centers enable dynamic electron transfer via 4f–5d orbitals, accelerating LiPSs redox kinetics, enhancing adsorption, and regulating Li+ deposition through local electric field modulation. Consequently, symmetric cells with this separator achieve ultralong stability over 3600 h at 1 mA cm–2/1 mAh cm–2, while full cells cycle stably over 600 cycles at 1 C with 0.040% per cycle capacity decay. This study offers a robust separator strategy to concurrently address polysulfide diffusion and lithium dendrite growth in high-performance LSBs.
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DOI
PubMed
高影响因子
Research
·
2020
·
IF 0
Jiapeng Ji,Ying Sha,Zeheng Li,Xuehui Gao,Teng Zhang,Shiyu Zhou,Tong Qiu,Shaodong Zhou,Liang Zhang,Min Ling,Yanglong Hou,Chengdu Liang
The shuttle effect hinders the practical application of lithium-sulfur (Li-S) batteries due to the poor affinity between a substrate and Li polysulfides (LiPSs) and the sluggish transition of soluble LiPSs to insoluble Li2S or elemental S. Here, we report that Ni hexatomic clusters embedded in a nitrogen-doped three-dimensional (3D) graphene framework (Ni-N/G) possess stronger interaction with soluble polysulfides than that with insoluble polysulfides. The synthetic electrocatalyst deployed in the sulfur cathode plays a multifunctional role: (i) selectively adsorbing the polysulfides dissolved in the electrolyte, (ii) expediting the sluggish liquid-solid phase transformations at the active sites as electrocatalysts, and (iii) accelerating the kinetics of the electrochemical reaction of multielectron sulfur, thereby inhibiting the dissolution of LiPSs. The constructed S@Ni-N/G cathode delivers an areal capacity of 9.43 mAh cm-2 at 0.1 C at S loading of 6.8 mg cm-2, and it exhibits a gravimetric capacity of 1104 mAh g-1 with a capacity fading rate of 0.045% per cycle over 50 cycles at 0.2 C at S loading of 2.0 mg cm-2. This work opens a rational approach to achieve the selective adsorption and expediting of polysulfide transition for the performance enhancement of Li-S batteries.
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DOI
ENERGY & FUELS
·
2024
·
IF 5.2
Ruoshan Jin,Zichun Xiao,Zhanhui Jia,Jiawu Cui,Chengyong Shu,Yu Bai,Wei Tang,Yuping Wu
It is still a huge challenge for lithium metal batteries (LMBs) with high energy density for practical application due to the intractable dendrite-growth issue triggered by inhomogeneous Li deposition as well as the unstable solid electrolyte interphase (SEI). For the purpose of constructing a dendrite-free Li metal anode, herein we designed and fabricated a functional separator (ZIF-L/rGO@PP) by facile vacuum infiltration in order to realize the effective regulation of ion transport. The nanochannels in ZIF-L with polar functional groups promote the uniform Li+ flux and the restricted migration of anions, while the rGO lamella endows the coating with good flexibility by reinforcing the interlayer bonding interactions. Based on the synergistic effects of ZIF-L and rGO, the functional separator exhibited superb electrolyte wettability and a high Li+ transference number of 0.66, ensuring the uniformity of Li+ transmission and thus induced a robust interface of the Li anode. Consequently, the cells with ZIF-L/rGO@PP separators delivered prolonged lifespan over 700 h with a small overpotential of less than 40 mV at 2 mA cm–2. More importantly, the employment of the separator enables Li||NCM811 full cell with enhanced cycling stability even under the limited N/P ratio of 2.5.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Pengfei Wan,Xincheng Guo,Shengdong Jing,Shilan Li,Shengjun Lu,Yufei Zhang,Haosen Fan
Lithium-sulfur (Li-S) batteries present tremendous potential in promising high energy storage systems because of their high energy density and specific capacity. However, the shuttle effect and slow reaction kinetics of the intermediate lithium polysulfide (LiPSs) result in fast capacity fading. Herein, multicomponent synergy nitrogen-doped carbon nanotube (CNT) framework dotted by CoFe/FeN 0.0324 /TiN heterostructure (CoFe/FeN 0.0324 /TiN@N-CNT) were developed and prepared by in-situ nitridation approach as polysulfide mediator to simultaneously realize physicochemical adsorption and catalytic conversion of polysulfide. Transition metal nitrides, such as FeN 0.0324 , are known for their polar surfaces that can chemically adsorb polysulfides efficiently. Additionally, CoFe and TiN have been shown to catalyze polysulfide redox reactions. This understanding paves the way for the development of heterostructured CoFe/FeN 0.0324 /TiN nanoparticles that significantly enhance the immobilization, diffusion, and transformation of polysulfides. Moreover, nitrogen-doped carbon nanotubes (CNTs) decorated with bimetallic CoFe afford intriguing benefits. The CoFe alloy not only facilitates the in-situ growth of CNTs but also contributes to prominent Li + /electron conductivity. Together, CoFe and CNTs provide substantial physical confinement and catalytic sites, thereby accelerating redox kinetics and effectively mitigating the shuttle effect. Owing to these advantages, CoFe/FeN 0.0324 /TiN@N-CNT separators exhibit remarkable electrochemical properties including superior rate capacity of 738 mAh g −1 at 3C, high reversible capacity of 708 mAh g −1 at 0.5C after 400 cycles and 607 mAh g −1 at 1C after 1000 cycles with per cycle declining rate of 0.09 % and 0.048 %, respectively, and ultralong cycle life at 4C after 1000 cycle. Even with a relatively high sulfur loading of 2.3 mg, the modified batteries still exhibit a satisfactory reversible capacity at 0.5C. This work paves a unique avenue combined prudent spacial framework with heterogeneous synergy strategy for manufacturing high-energy–density Li-S batteries.
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DOI
高影响因子
Energy & Environmental Materials
·
2023
·Vol. 7
·期 3
·e12648
·
IF 15
Yanan Li,Shunchao Ma,Yuehua Zhao,Silin Chen,Tingting Xiao,Hongxing Yin,Huiyu Song,Xiumei Pan,Lina Cong,Haiming Xie
High Li + transference number electrolytes have long been understood to provide attractive candidates for realizing uniform deposition of Li + . However, such electrolytes with immobilized anions would result in incomplete solid electrolyte interphase (SEI) formation on the Li anode because it suffers from the absence of appropriate inorganic components entirely derived from anions decomposition. Herein, a boron-rich hexagonal polymer structured all-solid-state polymer electrolyte (BSPE+10% LiBOB) with regulated intermolecular interaction is proposed to trade off a high Li + transference number against stable SEI properties. The Li + transference number of the as-prepared electrolyte is increased from 0.23 to 0.83 owing to the boron-rich cross-linker (BC) addition. More intriguingly, for the first time, the experiments combined with theoretical calculation results reveal that BOB − anions have stronger interaction with B atoms in polymer chain than TFSI − , which significantly induce the TFSI − decomposition and consequently increase the amount of LiF and Li 3 N in the SEI layer. Eventually, a LiFePO 4 |BSPE+10% LiBOB|Li cell retains 96.7% after 400 cycles while the cell without BC-resisted electrolyte only retains 40.8%. BSPE+10% LiBOB also facilitates stable electrochemical cycling of solid-state Li-S cells. This study blazes a new trail in controlling the Li + transport ability and SEI properties, synergistically.
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DOI
高影响因子
RSC Advances
·
2013
·Vol. 3
·期 32
·13149-13155
·
IF 2.562
Kunlei Zhu,Jianhua Tian,Yiping Liu,Na Lin,Qiwei Tang,Xiangmei Yu,Yingming Zhu,Zhongqiang Shan
The effect of reaction temperature and aging time on TiO2 precursor beads synthesized using a sol–gel method was studied. The size of the precursor beads decreased and deformed spheres appeared with increasing temperature. Meanwhile, TiO2 precursor beads grew with the aging time up to a reaction time of 18 h. Using a solvothermal process for the precursor beads, submicron-sized mesoporous anatase TiO2 beads (SMATBs) with a specific surface of 153.2 m2 g−1, much higher than initially reported, were synthesized by controlling the reaction conditions and were successfully employed as negative electrode for Li-ion batteries. The specific capacities of the submicron-sized mesoporous TiO2 beads are much higher than those of their counterparts at high charge–discharge rates. In the first cycle, the TiO2 beads showed discharge capacities of 172.0 mA h g−1, 129.6 mA h g−1, 117.1 mA h g−1 and 56.7 mA h g−1 at charge–discharge rates of 1 C (1 C = 170 mA g−1), 5 C, 10 C and 30 C, respectively. 85.1% discharge capacities were retained after 200 cycles at 1 C charge–discharge rate. After 600 cycles, there is still 81.8% discharge capacity retained at 5 C charge–discharge rate. Moreover, the TiO2 beads also exhibitied 86.9 mA h g−1 and 34.0 mA h g−1 discharge capacities at 10 C and 30 C charge–discharge rates over 600 cycles, respectively. In addition, the Coulombic efficiency is nearly 100% at each cycle at various charge–discharge rates.
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DOI
高影响因子
NANOTECHNOLOGY
·
2020
·Vol. 31
·期 33
·335403
·
IF 3.551
Yong Wu,Tianli Han,Ting Zhou,Xue Qiao,Xi Chen,Ping Zhou,Jinyun Liu
Conventional approaches for preparing yolk-shell nanostructures require complicated procedures such as multi-step coatings and template removal. Herein, we present a new and general strategy for making yolk-shell nanocomposites based on an oil-in-water emulsion system. As a demonstrating case, silicon nanoparticles were dispersed in an oil phase which was in an oil-in-water emulsion; then the oil/water interface was in-situ polymerized to form microcapsules. After carbonization, the shell of microcapsules was formed. The Li-ion battery anodes based on the microcapsules exhibit a good electrochemical performance including stable capacity and high rate-performance. The capacity remains 1100 mAh g−1 after 500 cycles at a current density of 1.9 A g−1, along with a Coulombic efficiency of ≈ 99.9%. In addition, the method presented here is general, which is applicable for the synthesis of many yolk shell-structured nanocomposites.
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Youshuang Zhou,JianYun Ding,Zhaoyang Wei,Weiwei Lei,Jun You,Qunchao Zhang,Dean Shi
The catalytic effect of zinc sulfide (ZnS) on the transformation of polysulfides (Li 2 S 8 ) to lithium sulfide (Li 2 S) has been proven by the enhancement in the rate performance of lithium-sulfur (Li–S) batteries incorporating ZnS particles into the cathode. Accordingly, the shuttling effect of polysulfide should also be suppressed. However, the expected phenomenon is not found in the Li–S batteries with ZnS particles being added in the cathodes. In order to find the intrinsic mechanism of this phenomenon, detailed catalytic effects of ZnS particles on different polysulfide molecules are investigated. It is shown that ZnS can only enhance the reaction from Li 2 S 4 to Li 2 S and it has almost no catalytic effect on the reaction from Li 2 S 6 to Li 2 S 4 . This is why the shuttle effect of Li 2 S 6 cannot be effectively prohibited. This mechanism is further verified via combining ZnS particles with S–C@PVA yolk-shell particles containing sulfur (S) and carbon black (C) as the core and PVA as the shell. Although the reaction from Li 2 S 6 to Li 2 S 4 cannot be directly catalysed by ZnS particles, it can still be enhanced when ZnS particles are distributed within the S–C@PVA yolk-shell structure (S–C–ZnS@PVA) because the reaction speed from the Li 2 S 4 to Li 2 S is accelerated. The fast consumption of Li 2 S 4 will result in the enhancement of the reaction from Li 2 S 6 to Li 2 S 4 , which will largely reduce the diffusion of Li 2 S 6 out of the PVA shell. While if ZnS particles are located outside the S–C@PVA yolk-shell structure (S–C@PVA-ZnS), large amount of Li 2 S 6 can still diffuse out of the PVA shell and enter into the electrolyte since the transformation from is Li 2 S 6 to Li 2 S 4 relatively low. Both the rate performance and cycle stability of the batteries with S–C–ZnS@PVA cathodes are higher than those with S–C@PVA-ZnS ones. These results will give a guidance for the preparation of Li–S battery with high performance.
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 54
·期 7
·5584-5594
·
IF 3.442
Lv Tingjian,Guan Li,Xiao Peng,Zhang Dongyun,Chang Chengkang
In this work, we report the preparation and the enhanced electrochemical performance of P2-type Na 0.67 Li x (Mn 0.5 Fe 0.25 Co 0.25 ) 1− x O 2 layered cathode materials with different Li substitutions via a nanomilling-assisted solid-state method. The experimental results show that the introduced lithium ions can greatly improve the performance of the material after entering the transition metal layer. Among these synthesized samples, the Na 0.67 Li 0.03 (Mn 0.5 Fe 0.25 Co 0.25 ) 0.97 O 2 electrode exhibits an exceptionally high specific capacity of 190.6 mAh g −1 at 0.1 C rate and a capacity retention of 89.5% after 30 cycles. Obviously, the specific capacity retention is improved by 15.3% compared with the pristine Na 0.67 (Mn 0.5 Fe 0.25 Co 0.25 )O 2 without Li incorporation (the specific capacity retention is only 74.2% after 30 cycles). Simultaneously, the sample also shows a large increase in rate performance compared to the pristine material. All of the enhancement can be explained by the fact that the introduced Li ions suppress the phase transition during the charge–discharge process and avoid the volume expansion of the electrode, which significantly reduce the occurrence of micro-cracks within the electrode. The reduced polarization, the decreased internal resistance of the prepared electrodes and the increased sodium ion diffusion coefficient, as confirmed from the CV and EIS measurements, can be regarded as the three major reasons for the enhanced electrochemical performance of the Li ion-substituted materials.
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DOI
高影响因子
Small
·
2021
·Vol. 17
·期 47
·2103830
·
IF 13.281
Xiaohua Li,Zhao Jiang,Dan Cai,Xiuli Wang,Xinhui Xia,Changdong Gu,Jiangping Tu
All-solid-state lithium batteries (ASSLBs) adopting sulfide electrolytes and high-voltage layered oxide cathodes have moved into the mainstream owing to their superior safety and immense potential in high energy density. However, the poor electrochemical compatibility between oxide cathodes and sulfide electrolytes remains a challenge for high-performance ASSLBs. In this study, a nanoscale Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 (LATP) phosphate coating is reasonably constructed on the surface of single-crystal LiNi 0.6 Co 0.2 Mn 0.2 O 2 particles to achieve cathode/electrolyte interfacial stability. The conformal LATP layer with inherent high-voltage stability can effectively suppress the oxidation decomposition of the electrolyte and demonstrate chemical inertness to both the oxide cathode and Li 10 SnP 2 S 12 electrolyte. ASSLBs with an LATP-modified cathode exhibited a high initial discharge capacity (152.1 mAh g −1 ), acceptable rate capability, and superior cycling performance with a capacity retention of 87.6% after 100 cycles at 0.1 C. Interfacial modification is an effective approach for achieving high-performance sulfide-based ASSLBs with superior interfacial stability.
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DOI
高影响因子
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